High-precision measurement of U-Pu-Np-Am concentrations and isotope ratios in environmental reference materials by mass spectrometry.
TL;DR: In this article, the authors report results of precise and sensitive mass spectrometric measurements of uranium, plutonium, neptunium, and americium concentrations and isotope ratios in a variety of environmental reference materials.
About: This article is published in Journal of Environmental Radioactivity.The article was published on 2021-10-01. It has received 5 citations till now. The article focuses on the topics: Isotopic signature & Isotope dilution.
Citations
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TL;DR: In this article , a simplified and very flexible chemical purification procedure based on extraction chromatography (a single UTEVA® column) was implemented which can be extended by a DGA® column for Am purification.
Abstract: Recent major advances in Accelerator Mass Spectrometry (AMS) at the Vienna Environmental Research Accelerator (VERA) regarding detection efficiency and isobar suppression have opened possibilities for the analysis of additional long-lived radionuclides at ultra-low environmental concentrations. These radionuclides, including 233U, 135Cs, 99Tc, and 90Sr, will become important for oceanographic tracer application due to their generally conservative behavior in ocean water. In particular, the isotope ratios 233U/236U and 137Cs/135Cs have proven to be powerful fingerprints for emission source identification as they are not affected by elemental fractionation. Improved detection efficiencies allowed us to analyze all major long-lived actinides, i.e., 236U, 237Np, 239,240Pu, 241Am as well as the very rare 233U, in the same 10 L water samples of a depth profile from the northwest Pacific Ocean. For this purpose, a simplified and very flexible chemical purification procedure based on extraction chromatography (a single UTEVA® column) was implemented which can be extended by a DGA® column for Am purification. The procedure was validated with the reference materials IAEA-381/385. With the additional increase in ionization efficiency expected for the extraction of actinides as fluoride molecules from the AMS ion source, a further reduction of chemical processing may become possible. This method was successfully applied to an exemplary set of air filter samples. In order to determine the quantitative 237Np concentration reliably, a 236Np spike material is being developed in collaboration with the University of Tsukuba, Japan. Ion-Laser Interaction Mass Spectrometry (ILIAMS), a novel technique for the efficient suppression of stable isobaric background, has been developed at VERA and provides unprecedented detection sensitivity for the fission fragments 135Cs, 99Tc, and 90Sr. The corresponding setup is fully operational now and the isobar suppression factors of >105 achieved, in principle, allow for the detection of the mentioned radionuclides in the environment. Especially for 90Sr analysis, this new approach has already been validated for selected reference materials (e.g., IAEA-A-12) and is ready for application in oceanographic studies. We estimate that a sample volume of only (1–3) L ocean water is sufficient for 90Sr as well as for 135Cs analysis, respectively.
9 citations
TL;DR: In this paper , the separation and measurement methods for ultra-trace determination of 90Sr, 239Pu, and 240Pu in the environment are discussed and compared, and the future development trend of radionuclide measurement is prospected in this review.
Abstract: Artificial long-lived radionuclides such as 90Sr and 239,240Pu have been long released into the environment by human nuclear activities, which have a profound impact on the ecological environment. It is of great significance to monitor the concentration of these radionuclides for environmental safety. This paper summarizes and critically discusses the separation and measurement methods for ultra-trace determination of 90Sr, 239Pu, and 240Pu in the environment. After selecting the measurement method, it is necessary to consider the decontamination of the interference from matrix elements and the key elements, and this involves the choice of the separation method. Measurement methods include both radiometric methods and non-radiometric methods. Radiometric methods, including alpha spectroscopy, liquid scintillation spectrometry, etc., are commonly used methods for measuring 239+240Pu and 90Sr. Mass spectrometry, as the representative of non-radiometric measurement methods, has been regarded as the most promising analytical method due to its high absolute sensitivity, low detection limit, and relatively short sample-analysis time. Through the comparison of various measurement methods, the future development trend of radionuclide measurement is prospected in this review. The fully automatic and rapid analysis method is a highlight. The new mass spectrometer with ultra-high sensitivity shows strong analytical capabilities for extremely low concentrations of 90Sr, 239Pu, and 240Pu, and it is expected to develop determination methods with higher sensitivity and lower detection limit.
2 citations
TL;DR: In this article , a simple and rapid chromatographic separation method for purposeful and efficient separation of 241Am from matrix and interfering elements was developed, which was finally applied to real marine sediment samples collected in the western North Pacific after the Fukushima nuclear accident.
1 citations
TL;DR: In this paper , a review covers advances in the analysis of air, water, plants, soils and geological materials by a range of atomic spectrometric techniques including atomic emission, absorption, fluorescence and mass spectrometry.
Abstract: This review covers advances in the analysis of air, water, plants, soils and geological materials by a range of atomic spectrometric techniques including atomic emission, absorption, fluorescence and mass spectrometry.
1 citations
TL;DR: In this paper , the authors compared the performance of inductively coupled plasma tandem mass spectrometers (ICP-MS/MS) for the detection of plutonium isotopes in a variety of soil types.
Abstract: Abstract The measurement of isotopic abundances and ratio variations of plutonium can provide important information about the sources and behaviours of radiogenic isotopes in the environment. The detection of ultra-trace isotopes of plutonium is increasing interest in the scientific literature for the determination of soil erosion rates due to their long retention times in the environment. The characteristics of plutonium within the environment make it an ideal tracer for the determination of soil redistribution rates and its robustness presents the opportunity to replace more commonly used radioisotopes such as 137 Cesium and 210 Lead. However, ultra-trace analysis of plutonium (fg g −1 ) presents analytical challenges which must be overcome in a variety of soil types. Inductively Coupled Plasma Mass Spectrometry has proven valuable for detection of plutonium in a range of environmental samples. However, severe polyatomic interferences from uranium isotopes significantly limits its application. Due to the improvements in detection sensitivity and reaction cell technology, inductively coupled plasma tandem mass spectrometry, which is also commonly referred to as triple quadrupole inductively coupled plasma tandem mass spectrometry (ICP-MS/MS), has emerged as an exceptional tool for ultra-trace elemental analysis of plutonium isotopes in environmental samples overcoming the limitations of standard quadrupole ICP-MS such as limited sensitivity and cost of analysis. In this review, common methods reported in the literature for the separation and subsequent detection of plutonium isotopes are compared to recent advances in analysis using ICP-MS/MS technology. Graphical Abstract
References
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TL;DR: New determinations of the half-lives of half-life values of $ −235 and −238 have been made improved techniques have allowed the halflife values to be measured with greater accuracy than has been heretofore achieved as discussed by the authors.
Abstract: New determinations of the half-lives of $^{235}\mathrm{U}$ and $^{238}\mathrm{U}$ have been made Improved techniques have allowed the half-life values to be measured with greater accuracy than has been heretofore achieved Samples were prepared by molecular plating and counted in a intermediate-geometry $\ensuremath{\alpha}$-proportional counter with an extremely flat pulse-height plateau The small amount of residual nonplated uranium was counted in a $2\ensuremath{\pi}$ counter Energy analysis with a silicon-junction detector was used to measure the presence of "foreign" activities For $^{235}\mathrm{U}$, the measured specific activity was (47981\ifmmode\pm\else\textpm\fi{}33) (dis/min)/(mg $^{235}\mathrm{U}$), corresponding to a half-life of (70381\ifmmode\pm\else\textpm\fi{}00048) \ifmmode\times\else\texttimes\fi{} ${10}^{8}$ yr For $^{238}\mathrm{U}$, the specific activity was measured as (74619\ifmmode\pm\else\textpm\fi{}041) (dis/min)/(mg $^{238}\mathrm{U}$), corresponding to a half-life of (44683\ifmmode\pm\else\textpm\fi{}00024) \ifmmode\times\else\texttimes\fi{} ${10}^{9}$ yr Errors quoted are statistical (standard error of the mean), based upon the observed scatter of the data This scatter exceeds that expected from counting statistics alone We believe that systematic errors, if present, will no more than double the quoted errors
2,543 citations
TL;DR: In this article, the authors used high precision thermal ionization mass spectrometric (TIMS) methods to determine the half-life of zircons with concordant 238 U/ 238 U and 230 Th / 238 U atomic ratios.
1,171 citations
TL;DR: From the results, it is concluded that fallout 237Np/239Pu atom ratios are generally lower in the Southern Hemisphere than in the Northern Hemisphere, and 237NP/ 239Puatom ratios are more device-dependent, hence more variable, than counterpart 240Pu/239Np atom ratios.
413 citations
TL;DR: In this article, the authors present new reference values for nineteen USGS, GSJ and GIT-IWG rock reference materials that belong to the most accessed samples of the GeoReM database.
Abstract: We present new reference values for nineteen USGS, GSJ and GIT-IWG rock reference materials that belong to the most accessed samples of the GeoReM database. The determination of the reference values and their uncertainties at the 95% confidence level follows as closely as possible ISO guidelines and the Certification Protocol of the International Association of Geoanalysts. We used analytical data obtained by the state-of-the-art techniques published mainly in the last 20 years and available in GeoReM. The data are grouped into four categories of different levels of metrological confidence, starting with isotope dilution mass spectrometry as a primary method. Data quality was checked by careful investigation of analytical procedures and by the application of the Horwitz function. As a result, we assign a new and more reliable set of reference values and respective uncertainties for major, minor and a large group of trace elements of the nineteen investigated rock reference materials.
325 citations